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Accelerated Reactions in Droplets and Thin Films: Surface Effects and Analytical Implications

液滴和薄膜中的加速反应：表面效应和分析意义

基本信息

批准号：
1905087
负责人：
Robert Cooks
金额：
$ 46.75万
依托单位：
Purdue University
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2019
资助国家：
美国
起止时间：
2019-08-15 至 2023-07-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1905087&HistoricalAwards=false
关键词：
Accelerated Reactions Droplets Thin Films

项目摘要

With support from the Chemical Measurement and Imaging Program in the Division of Chemistry, Professor Graham Cooks and his group at Purdue University are working to explain and exploit a startling but simple fact: the speed of many chemical reactions increases dramatically as the volume of the reacting mixture decreases. Because of this, reactions in microdroplets can easily be thousands of times faster than the same reactions in jars, barrels or industrial vats. This may offer an alternative to the use of expensive chemical catalysts to save time and energy. Research in the Cooks group is focused on understanding the role of the droplet interface in accelerating reactions, particularly those that are useful in various analytical measurements. Among other potential applications are studies of the shelf life of pharmaceuticals, and detailed examination of fast biochemical reactions that occur within living cells. The project provides training in advanced instrumentation and precision chemical measurements, and prepares graduate students to contribute to the US workforce in a field with strong industrial and national security ties. A range of methods will be deployed to transfer the results of the research and strengthen the training aspect of the program, including strong industrial interactions, focused short training courses, inclusion of undergraduates in research, and collaborative research efforts involving regional institutions with strength in analytical chemistry.The research objectives of this proposal are to discover and characterize ways to exploit accelerated reactions (including derivatization) for chemical analysis in droplets and other confined volumes, and to elucidate the mechanisms that increase reaction rate constants. The search for mechanistic knowledge focusses on kinetic studies of surface vs. bulk reactions as a function of droplet size and reagent concentration. Mass spectrometry can benefit from as well as probe these reactions. It is the main measurement tool, along with interfacial vibrational spectrometry. Other target applications come from both academic and industrial settings. Examples include chemical reactions involving non-covalent clusters of amino acids and peptide bond formation.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

在化学系化学测量和成像项目的支持下，普渡大学格雷厄姆·库克斯教授和他的团队正在努力解释和利用一个令人震惊但简单的事实：随着反应混合物体积的减小，许多化学反应的速度急剧增加。因此，微滴中的反应很容易比罐子、桶或工业桶中的相同反应快数千倍。这可能为使用昂贵的化学催化剂提供一种替代方案，以节省时间和能源。库克斯小组的研究重点是了解液滴界面在加速反应中的作用，特别是那些在各种分析测量中有用的反应。其他潜在的应用包括药物保质期的研究以及活细胞内发生的快速生化反应的详细检查。该项目提供先进仪器和精密化学测量方面的培训，并帮助研究生做好准备，在与工业和国家安全关系密切的领域为美国劳动力做出贡献。将采用一系列方法来转移研究成果并加强该计划的培训方面，包括强有力的工业互动、集中的短期培训课程、让本科生参与研究以及涉及具有分析化学实力的区域机构的合作研究工作。该提案的研究目标是发现和表征利用加速反应（包括衍生化）进行液滴和其他密闭化学分析的方法。体积，并阐明增加反应速率常数的机制。对机械知识的探索集中于表面反应与本体反应的动力学研究，作为液滴尺寸和试剂浓度的函数。质谱分析可以从这些反应中受益并对其进行探测。它与界面振动光谱测量一样是主要的测量工具。其他目标应用程序来自学术和工业环境。例子包括涉及氨基酸非共价簇和肽键形成的化学反应。该奖项反映了 NSF 的法定使命，并通过使用基金会的智力价值和更广泛的影响审查标准进行评估，被认为值得支持。

项目成果

期刊论文数量（28）

专著数量（0）

科研奖励数量（0）

会议论文数量（0）

专利数量（0）

Pd Reaction Intermediates in Suzuki‐Miyaura Cross‐Coupling Characterized by Mass Spectrometry

铃木钯反应中间体——宫浦十字——质谱表征的耦合

DOI：
10.1002/cplu.202100545
发表时间：
2022
期刊：
ChemPlusChem
影响因子：
3.4
作者：
Chen, Xingshuo;Wei, Zhenwei;Huang, Kai‐Hung;Uehling, Mycah;Wleklinski, Michael;Krska, Shane;Makarov, Alexey A.;Nowak, Timothy;Cooks, R. Graham
通讯作者：
Cooks, R. Graham

Mass spectrometry in materials synthesis

材料合成中的质谱分析